Attosecond vacuum UV coherent control of molecular dynamics

High harmonic light sources make it possible to access attosecond timescales, thus opening up the prospect of manipulating electronic wave packets for steering molecular dynamics. However, two decades after the birth of attosecond physics, the concept of attosecond chemistry has not yet been realize...

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Bibliographic Details
Published in:Proceedings of the National Academy of Sciences - PNAS 2014-01, Vol.111 (3), p.912-917
Main Authors: Ranitovic, Predrag, Hogle, Craig W., Rivière, Paula, Palacios, Alicia, Tong, Xiao-Ming, Toshima, Nobuyuki, González-Castrillo, Alberto, Martin, Leigh, Martín, Fernando, Murnane, Margaret M., Kapteyn, Henry
Format: Article
Language:English
Subjects:
Chemical reactions
Chemistry
Electrons
Harmonics
Infrared radiation
Ionization
Lasers
Molecules
Photons
Physical Sciences
Ultraviolet radiation
Wave excitation
Wave packets
Wavelengths
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Summary:High harmonic light sources make it possible to access attosecond timescales, thus opening up the prospect of manipulating electronic wave packets for steering molecular dynamics. However, two decades after the birth of attosecond physics, the concept of attosecond chemistry has not yet been realized; this is because excitation and manipulation of molecular orbitals requires precisely controlled attosecond waveforms in the deep UV, which have not yet been synthesized. Here, we present a unique approach using attosecond vacuum UV pulse-trains to coherently excite and control the outcome of a simple chemical reaction in a deuterium molecule in a non-Born–Oppenheimer regime. By controlling the interfering pathways of electron wave packets in the excited neutral and singly ionized molecule, we unambiguously show that we can switch the excited electronic state on attosecond timescales, coherently guide the nuclear wave packets to dictate the way a neutral molecule vibrates, and steer and manipulate the ionization and dissociation channels. Furthermore, through advanced theory, we succeed in rigorously modeling multiscale electron and nuclear quantum control in a molecule. The observed richness and complexity of the dynamics, even in this very simplest of molecules, is both remarkable and daunting, and presents intriguing new possibilities for bridging the gap between attosecond physics and attochemistry.
ISSN:0027-8424
1091-6490
DOI:10.1073/pnas.1321999111